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All sourcesNASA NTRSDOE OSTI
NASA NTRS1961

Atmospheric Photochemistry

The upper atmosphere offers a vast photochemical laboratory free from solid surfaces, so all reactions take place in the gaseous phase. At 30 km altitude the pressure has fallen to about one-hundredth of that at ground level, and we shall, rather arbitrarily, regard the upper atmosphere as beginning at that height. By a little less than 100 km the pressure has fallen to 10(exp -3) mm Hg and is decreasing by a power of ten for every 15 km increase in altitude. Essentially we are concerned then with the photochemistry of a nitrogen-oxygen mixture under low-pressure conditions in which photo-ionization, as well as photodissociation, plays an important part. Account must also be taken of the presence of rare constituents, such as water vapour and its decomposition products, including particularly hydroxyl, oxides of carbon, methane and, strangely enough, sodium, lithium and calcium. Many curious and unfamiliar reactions occur in the upper atmosphere. Some of them are luminescent, causing the atmosphere to emit a dim light called the airglow. Others, between gaseous ions and neutral molecules, are almost a complete mystery at this time. Similar interesting phenomena must occur in other planetary atmospheres, and they might be predicted if sufficient chemical information were available.

Massey, Harrie↗
NASA NTRS2008

Detection of Abiotic Methane in Terrestrial Continental Hydrothermal Systems: Implications for Methane on Mars

The recent detection of methane in the Martian atmosphere and the possibility that its origin could be attributed to biological activity, have highlighted the importance of understanding the mechanisms of methane formation and its usefulness as a biomarker. Much debate has centered on the source of the methane in hydrothermal fluids, whether it is formed biologically by microorganisms, diagenetically through the decomposition of sedimentary organic matter, or inorganically via reduction of CO2 at high temperatures. Ongoing research has now shown that much of the methane present in sea-floor hydrothermal systems is probably formed through inorganic CO2 reduction processes at very high temperatures (greater than 400 C). Experimental results have indicated that methane might form inorganically at temperatures lower still, however these results remain controversial. Currently, methane in continental hydrothermal systems is thought to be formed mainly through the breakdown of sedimentary organic matter and carbon isotope equilibrium between CO2 and CH4 is thought to be rarely present if at all. Based on isotopic measurements of CO2 and CH4 in two continental hydrothermal systems, we suggest that carbon isotope equilibration exists at temperatures as low as 155 C. This would indicate that methane is forming through abiotic CO2 reduction at lower temperatures than previously thought and could bolster arguments for an abiotic origin of the methane detected in the martian atmosphere.

Socki, Richard A.↗
NASA NTRS2015

Evaluation of Volatile Species in Green Monopropellant Project

NASA is interested in green monopropellants to replace hydrazine in reaction control systems (RCSs). Some current NASA programs require reduced vapor pressure and low toxicity monopropellant (green) and superior performance (specific impulse and density) formulations. Earlier vapor phase studies of a candidate green monopropellant at the NASA White Sands Test Facility (WSTF) showed the presence of a volatile species that warranted further investigation. The purpose of this study was to further characterize the volatile species and to evaluate it. The evaluation was with respect to whether the volatile species was an impurity or how it is formed, and to use that information to examine whether its presence as an impurity can be eliminated during formulation. The evaluation also considered whether formation of the volatile impurity could be prevented while not compromising the propellant. To reduce variables associated with evaluation of the propellant formulation as a whole, a precursor to one of the individual components in the propellant formulation was subjected to a NASA Standard 6001B Flammability, Off-gassing, and Compatibility Requirements and Test Procedures "Determination of Off-gassed Products (Test 7)". Testing took place in the NASA WSTF Molecular Desorption and Analysis Laboratory. One gram of the precursor was placed in a flask within a specimen container. After thermal conditioning for 72 +/- 1 h at 50 +/- 3 deg C (122 +/- 5 deg F), the atmosphere inside the specimen container was analyzed for off-gassed compounds by cryotrap gas chromatography-mass spectrometry (GC-MS) and fixed sample loop GC-flame ionization detection (GC-FID). The specimen container used was glass to minimize potential catalytic surfaces. The identification of compounds was difficult due to the complexity of the vapor phase concentrations and overlapping chromatographic peaks and mass spectra. However, eleven compounds were specifically identified and five compounds or classes of compounds were reported as unidentified. Quantitation of most of the compounds, including unidentified compounds, was as methane. Quantitating compounds or classes of compounds that were detected but for which specific calibration is not established as methane is in accordance with the Test 7 standard protocol. The thermal decomposition temperature of the precursor was significantly higher than the test temperature. Based on thermal decomposition temperature and on an examination of the structure and chemistry of the identified volatile species, the presence of the volatile species appears to be chemically reasonable with respect to the propellant formulation and is at this time attributed to impurities. Further examination of the overall propellant formulation process (including the individual components' synthesis processes) and process quality control (including purity of reagents and possible decomposition reactions) is indicated.

Greene, Benjamin↗
NASA NTRS2005

High-temperature catalyst for catalytic combustion and decomposition

A robust, high temperature mixed metal oxide catalyst for propellant composition, including high concentration hydrogen peroxide, and catalytic combustion, including methane air mixtures. The uses include target, space, and on-orbit propulsion systems and low-emission terrestrial power and gas generation. The catalyst system requires no special preheat apparatus or special sequencing to meet start-up requirements, enabling a fast overall response time. Start-up transients of less than 1 second have been demonstrated with catalyst bed and propellant temperatures as low as 50 degrees Fahrenheit. The catalyst system has consistently demonstrated high decomposition effeciency, extremely low decomposition roughness, and long operating life on multiple test particles.

Mays, Jeffrey A.↗
NASA NTRS2004

A Simulation Model of Carbon Cycling and Methane Emissions in Amazon Wetlands

An integrative carbon study is investigating the hypothesis that measured fluxes of methane from wetlands in the Amazon region can be predicted accurately using a combination of process modeling of ecosystem carbon cycles and remote sensing of regional floodplain dynamics. A new simulation model has been build using the NASA- CASA concept for predicting methane production and emission fluxes in Amazon river and floodplain ecosystems. Numerous innovations area being made to model Amazon wetland ecosystems, including: (1) prediction of wetland net primary production (NPP) as the source for plant litter decomposition and accumulation of sediment organic matter in two major vegetation classes - flooded forests (varzea or igapo) and floating macrophytes, (2) representation of controls on carbon processing and methane evasion at the diffusive boundary layer, through the lake water column, and in wetland sediments as a function of changes in floodplain water level, (3) inclusion of surface emissions controls on wetland methane fluxes, including variations in daily surface temperature and of hydrostatic pressure linked to water level fluctuations. A model design overview and early simulation results are presented.

Potter, Christopher↗
NASA NTRS2015

The Relative Importance of Methanogenesis in the Decomposition of Organic Matter in Northern Peatlands

Using an isotope-mass balance approach and assuming the equimolar production of CO2 and CH4 from methanogenesis (e.g., anaerobic decomposition of cellulose), we calculate that the proportion of total CO2 production from methanogenesis varies from 37 to 83% across a variety of northern peatlands. In a relative sense, methanogenesis was a more important pathway for decomposition in bogs (80 +/- 13% of CO2 production) than in fens (64 +/- 5.7% of CO2 production), but because fens contain more labile substrates they may support higher CH4 production overall. The concentration of CO2 produced from methanogenesis (CO2-meth) can be considered equivalent to CH4 concentration before loss due to ebullition, plant-mediated transport, or diffusion. Bogs produced slightly less CO2-meth than fens (2.9 +/- 1.3 and 3.7 +/- 1.4 mmol/L, respectively). Comparing the quantity of CH4 present to CO2-meth, fens lost slightly more CH4 than bogs (89 +/- 2.8% and 82 +/- 5.3%, respectively) likely due to the presence of vascular plant roots. In collapsed permafrost wetlands, bog moats produced half the amount of CO2-meth (0.8 +/- 0.2mmol/L) relative to midbogs (1.6 +/- 0.6 mmol/L) and methanogenesis was less important (42 +/- 6.6% of total CO2 production relative to 55 +/- 8.1%).We hypothesize that the lower methane production potential in collapsed permafrost wetlands occurs because recently thawed organic substrates are being first exposed to the initial phases of anaerobic decomposition following collapse and flooding. Bog moats lost a comparable amount of CH4 as midbogs (63 +/- 7.0% and 64 +/- 9.3%).

bacteria↗
NASA NTRS1990

Radiolysis of aqueous solutions of acetic acid in the presence of Na-montmorillonite

The gamma-irradiation of 0.8 mol dm-3 aqueous, oxygen-free acetic acid solutions was investigated in the presence or absence of Na-montmorillonite. H2, CH4, CO, CO2, and several polycarboxylic acids were formed in all systems. The primary characteristics observed in the latter system were: (1) Higher yield of the decomposition of acetic acid; (2) Lower yield of the formation of polycarboxylic acids; (3) No effect on the formation of methane; (4) Higher yield of the formation of carbon dioxide; and (5) The reduction of Fe3+ in the octahedral sites of Na-montmorillonite. A possible reaction scheme was proposed to account for the observed changes. The results are important in understanding heterogeneous processes in radiation catalysis and might be significant to prebiotic chemistry.

Non-NASA Center↗
NASA NTRS1999

Abiotic formation of hydrocarbons and oxygenated compounds during thermal decomposition of iron oxalate

The formation of organic compounds during the decomposition of iron oxalate dihydrate (IOD) was investigated as a possible analog for abiotic organic synthesis in geological systems. After heating at 330 degrees C for 2-4 days, IOD decomposed to a mixture of the minerals siderite and magnetite plus gas and non-volatile organic compounds. The organic products included an extremely large variety of compounds, making identification of individual reaction products difficult. However, the non-volatile products were dominated by several homologous series of alkylated cyclic compounds mostly containing a single aromatic ring, including alkylphenols, alkylbenzenes, alkyltetrahydronaphthols, and alkyltetrahydronaphthalenes. Traces of n-alkanols, n-alkanoic acids, n-alkanones, and n-alkanes were also identified. Carbon in the gas phase was predominantly CO2 (+CO?), with lesser amounts of light hydrocarbons to > C6 including all possible branched and normal isomers of the alkanes and alkenes. The organic products were apparently the result of two concurrent reaction processes: (1) condensation of the two-carbon units present in the initial oxalate moiety, and (2) Fischer-Tropsch-type synthesis from CO2 or CO generated during the experiment. Compounds produced by the former process may not be characteristic of synthesis from the single-carbon precursors which predominate in geologic systems, suggesting iron oxalate decomposition may not provide a particularly suitable analog for investigation of abiotic organic synthesis. When water was included in the reaction vessels, CO2 and traces of methane and light hydrocarbon gases were the only carbon products observed (other than siderite), suggesting that the presence of water allowed the system to proceed rapidly towards equilibrium and precluded the formation of metastable organic intermediates.

Non-NASA Center↗
NASA NTRS1981

Molecular carbon isotopic evidence for the origin of geothermal hydrocarbons

Isotopic measurements of individual geothermal hydrocarbons that are, as a group, of higher molecular weight than methane are reported. It is believed in light of this data that the principal source of hydrocarbons in four geothermal areas in western North America is the thermal decomposition of sedimentary or groundwater organic matter.

Des Marais, D. J.↗
NASA NTRS2001

Initiation of Martian Outflow Channels: Related to the Dissociation of Gas Hydrate?

We propose that the disruption of subpermafrost aquifers on Mars by the thermal- or pressure-induced dissociation of methane hydrate may have been a frequent trigger for initiating outflow channel activity. This possibility is raised by recent work that suggests that significant amounts of methane and gas hydrate may have been produced within and beneath the planet's cryosphere. On Earth, the build-up of overpressured water and gas by the decomposition of hydrate deposits has been implicated in the formation of large blowout features on the ocean floor. These features display a remarkable resemblance (in both morphology and scale) to the chaotic terrain found at the source of many Martian channels. The destabilization of hydrate can generate pressures sufficient to disrupt aquifers confined by up to 5 kilometers of frozen ground, while smaller discharges may result from the water produced by the decomposition of near-surface hydrate alone.

Max, Michael D.↗
NASA NTRS2013

Isotopic and Geochemical Investigation of Two Distinct Mars Analog Environments Using Evolved Gas Techniques in Svalbard, Norway

The 2010 Arctic Mars Analog Svalbard Expedition (AMASE) investigated two distinct geologic settings on Svalbard, using methodologies and techniques to be deployed on Mars Science Laboratory (MSL). AMASErelated research comprises both analyses conducted during the expedition and further analyses of collected samples using laboratory facilities at a variety of institutions. The Sample Analysis at Mars (SAM) instrument suite on MSL includes pyrolysis ovens, a gas-processing manifold, a quadrupole mass spectrometer (QMS), several gas chromatography columns, and a Tunable Laser Spectrometer (TLS). An integral part of SAM development is the deployment of SAM-like instrumentation in the field. During AMASE 2010, two parts of SAM participated as stand-alone instruments. A Hiden Evolved Gas Analysis- Mass Spectrometer (EGA-QMS) system represented the EGA-QMS component of SAM, and a Picarro Cavity Ring Down Spectrometer (EGA-CRDS), represented the EGA-TLS component of SAM. A field analog of CheMin, the XRD/XRF on MSL, was also deployed as part of this field campaign. Carbon isotopic measurements of CO2 evolved during thermal decomposition of carbonates were used together with EGA-QMS geochemical data, mineral composition information and contextual observations made during sample collection to distinguish carbonates formation associated with chemosynthetic activity at a fossil methane seep from abiotic processes forming carbonates associated with subglacial basaltic eruptions. Carbon and oxygen isotopes of the basalt-hosted carbonates suggest cryogenic carbonate formation, though more research is necessary to clarify the history of these rocks.

Svalbard↗
NASA NTRS1986

Oxidation and reduction rates for organic carbon in the Amazon mainstream tributary and floodplain, inferred from distributions of dissolved gases

Concentrations of CO2, O2, CH4, and N2O in the Amazon River system reflect an oxidation-reduction sequence in combination with physical mixing between the floodplain and the mainstem. Concentrations of CO2 ranged from 150 microM in the Amazon mainstem to 200 to 300 microM in aerobic waters of the floodplain, and up to 1000 microM in oxygen-depleted environments. Apparent oxygen utilization (AOU) ranged from 80 to 250 microM. Methane was highly supersaturated, with concentrations ranging from 0.06 microM in the mainstem to 100 microM on the floodplain. Concentrations of N2O were slightly supersaturated in the mainstem, but were undersaturated on the floodplain. Fluxes calculated from these concentrations indicated decomposition of 1600 g C sq m y(-1) of organic carbon in Amazon floodplain waters. Analysis of relationships between CH4, O2, and CO2 concentrations indicated that approximately 50 percent of carbon mineralization on the floodplain is anaerobic, with 20 percent lost to the atmoshphere as CH4. The predominance of anaerobic metabolism leads to consumption of N2O on the flood plane. Elevated concentrations of CH4 in the mainstem probably reflect imput from the floodplain, while high levels of CO2 in the mainstem are derived from a combination of varzea drainage and in situ respiration.

Richey, Jeffrey E.↗
NASA NTRS1981

Photolysis of CH4-NH3 mixtures and PH3 as models for the photochemical transformations on the primitive earth and Jupiter

Methane, ammonia and phosphine are some of the possible constituents of the atmospheres of the Jovian planets and their satellites. Photolysis of NH3 in the presence of CH4 at 185 nm in the temperature range of 25 C to -100 C results in the decomposition of CH4. The reaction is inhibited by added H2 or SF6. These findings are consistent with the reaction of hot hydrogen atoms with CH4 to give the CH3 radical. P2H4 is the initial product formed by the photolysis of PH3 at 206 nm. Kinetic studies established that it is the intermediate in the formation of P4 from PH3. The potential significance of these reactions to the atmospheric photochemistry of the Jovian planets and moons is discussed.

Ferris, J. P.↗
NASA NTRS1997

An Ecosystem Simulation Model for Methane Production and Emission from Wetlands

Previous experimental studies suggest that methane emission from wetland is influenced by multiple interactive pathways of gas production and transport through soil and sediment layers to the atmosphere. The objective of this study is to evaluate a new simulation model of methane production and emission in wetland soils that was developed initially to help identify key processes that regulate methanogenesis and net flux of CH4 to the air, but which is designed ultimately for regional simulation using remotely sensed inputs for land cover characteristics. The foundation for these computer simulations is based on a well-documented model (CASA) of ecosystem production and carbon cycling in the terrestrial blaspheme. Modifications to represent flooded wetland soils and anaerobic decomposition include three new sub-models for: (1) layered soil temperature and water table depth (WTD) as a function of daily climate drivers, (2) CH4 production within the anoxic soil layer as a function of WTD and CO2 production under poorly drained conditions, and (3) CH4 gaseous transport pathways (molecular diffusion, ebullition, and plant vascular transport) as a function of WTD and ecosystem type. The model was applied and tested using climate and ecological data to characterize tundra wetland sites near Fairbanks, Alaska studied previously by Whalen and Reeburgh. Comparison of model predictions to measurements of soil temperature and thaw depth, water-table depth, and CH4 emissions over a two year period suggest that inter-site differences in soil physical conditions and methane fluxes could be reproduced accurately for selected periods. Day-to-day comparison of predicted emissions to measured CH4 flux rates reveals good agreement during the early part of the thaw season, but the model tends to underestimate production of CH4 during the months of July and August in both test years. Important seasonal effects, including that of falling WTD during these periods, are apparently overlooked in the model formulation. Nevertheless, reasonably close agreement was achieved between the model's mean daily and seasonal estimates of CH4 flux and observed emission rates for northern wetland ecosystems. Several features of the model are identified as crucial to more accurate prediction of wetland methane emission, including the capacity to incorporate influences of localized topographic and hydrologic features on site-specific soil temperature and WTD dynamics, and mechanistic simulation of methane emission transport pathways from within the soil profile.

Potter, C. S.↗
NASA NTRS1991

Sources and geochemical evolution of cyanide and formaldehyde

The major source of cyanide has, in current paleoatmospheric models, been assumed to be the reaction of photodissociated thermospheric nitrogen with a limiting supply of stratospheric methane. Formaldehyde may be produced with more ease from an atmosphere of carbon dioxide as the dominant carbon species, and from carbonate in solution or sorbed in double layer hydroxide minerals. Potentially more important sources for cyanide and other carbon containing molecules are the partially photoprotected northern and southern auroral ovals where continuous currents reaching several mega-amperes induce ion-molecule reactions, extending into the lower stratosphere. In simulated environments of this kind, the cyanide ion is known to be produced from oxidized carbon species potentially more abundant than methane. Rainout of cyanide and formaldehyde place them in two different geochemical reaction reservoirs. In the anoxic Archean hydrosphere, about 1mM in Fe2(+), the cyanide ion would have been efficiently converted to the stable ferrocyanide complex Fe(CN) sub 6(4-), protecting it from the commonly considered fate of decomposition by hydrolysis, and eventually incorporating it in pyroaurite type minerals, most efficiently in green rust where it converts to insoluble ferriferrocyanide, prussian blue.

Arrhenius, G.↗
NASA NTRS1997

Stability of Trifluoromethane in Forest Soils and Methanotrophic Cultures

Trifluoromethane (TFM) has been reported as an endproduct of trifluoroacetate degradation under oxic conditions. Although other halomethanes, such as chloroform, methyl bromide, and methyl fluoride, inhibit methane oxidation or are degraded by methanotrophs, the fate of TFM is unknown. TFM had no affect on atmospheric methane consumption when added to forest soils at either 10 ppm or 10,000 ppm. No degradation of TFM was observed at either concentration for incubations of 6 days. Cultures of Methylobacter albus BG8 and Methylosinus trichosporium OB3b grown With and without added copper were also used to assay TFM degradation at 10 10000 ppm levels. TFM did not inhibit methane oxidation under any growth conditions, including those inducing expression of soluble methane monooxygenase, nor was it degraded at measurable rates. In contrast, parallel assays showed that both methyl fluoride and chloroform inhibited methane oxidation in M. trichosporium OB3b. Our results suggest that TFM may be relatively inert with respect to methanotrophic degradition. Although TFM has a negligible ozone depletion potential, it absorbs infrared radiation and has a relatively long atmospheric residence time. Thus, accumulation of TFM in the atmosphere as a consequence of the decomposition of hydrochlorofluorocarbons may have significant unpredicted climate impacts.

King, Gary M.↗
NASA NTRS1985

Multiplex gas chromatography for use in space craft

Gas chromatography is a powerful technique for the analysis of gaseous mixtures. Some limitations in this technique still exist which can be alleviated with multiplex gas chromatography (MGC). In MGC, rapid multiple sample injections are made into the column without having to wait for one determination to be finished before taking a new sample. The resulting data must then be reduced using computational methods such as cross correlation. In order to efficiently perform multiplexgas chromatography, experiments in the laboratory and on board future space craft, skills, equipment, and computer software were developed. Three new techniques for modulating, i.e., changing, sample concentrations were demonstrated by using desorption, decomposition, and catalytic modulators. In all of them, the need for a separate gas stream as the carrier was avoided by placing the modulator at the head of the column to directly modulate a sample stream. Finally, the analysis of an environmental sample by multiplex chromatography was accomplished by employing silver oxide to catalytically modulate methane in ambient air.

Valentin, J. R.↗
NASA NTRS1981

Irradiation of NH3-CH4 mixtures as a model of photochemical processes in the Jovian planets and Titan

The reactions occurring upon the ultraviolet irradiation of ammonia-methane mixtures are investigated in a simulation of the atmospheric chemistry of the Jovian planets and Titan. Gas mixtures were irradiated at 185 nm at temperatures from 156-298 K, and product and reactant concentrations were determined by means of gas chromatography. The ratio of the moles of CH4 lost per mole of NH3 decomposed is found to be 0.25, with the extent of CH4 decomposition independent of temperature. The absence of a temperature effect suggests that nonthermal atoms, probably hydrogen, initiate CH4 decomposition by the extraction of a hydrogen atom. A decrease in CH4 loss with increasing pressure or the addition of other gases to the photolysis mixture, and the lack of an increase in NH3 photolysis with CH4 pressure support this mechanism. Major reaction products obtained include C2H2, C3H8 or CH3NH2, and C4H10. Considerations of atmospheric concentrations of H2 and He indicate that NH3 photolysis does not contribute to CH4 decomposition on Jupiter, Saturn, Uranus, and Neptune, although it may have had a role in the formation of the Titan atmosphere.

Ferris, J. P.↗